Basic metal carbonate supported gold nanoparticles: enhanced performance in aerobic alcohol oxidation

Yang, Jingguo; Guan, Yejun; Verhoeven, Tiny; Santen, Rutger A. van; Li, Can; Hensen, Ejm Emiel

doi:10.1039/b821586c

Cited by 53 publications

(47 citation statements)

References 19 publications

(5 reference statements)

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“…Besides gas-phase CO oxidation, gold catalysts have also been reported to be excellent catalyst for selective oxidation of alcohols with molecular oxygen [2,42,74]. Table 5 includes the TOFs of the fresh catalysts based on the amount of benzylic alcohol converted and the total amount of gold.…”

Section: Resultsmentioning

confidence: 99%

“…Indeed, very often a soluble base is added to facilitate this reaction [80]. The support may also act as a base [42]. In the absence of a base, O-H bond activation may be slow and, in such case, surface oxygen atoms may facilitate this process.…”

Section: Discussionmentioning

confidence: 99%

“…The aerobic oxidation of benzyl alcohol was carried out as previously reported [42]. A round-bottle flask (25 mL) was charged with 100 mg of catalyst, 1 mmol of benzyl alcohol and 9.9 mL of toluene.…”

Section: Catalytic Activity Measurementsmentioning

confidence: 99%

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Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

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The interaction of gold atoms with CeO 2 nanocrystals having rod and cube shapes has been examined by cyanide leaching, TEM, TPR, CO IR and X-ray absorption spectroscopy. After deposition-precipitation and calcination of gold, these surfaces contain gold nanoparticles in the range 2-6 nm. For the ceria nanorods, a substantial amount of gold is present as cations that replace Ce ions in the surface as follows from their first and second coordination shells of oxygen and cerium by EXAFS analysis. These cations are stable against cyanide leaching in contrast to gold nanoparticles. Upon reduction the isolated Au atoms form finely dispersed metal clusters with a high activity in CO oxidation, the WGS reaction and 1,3-butadiene hydrogenation. By analogy with the very low activity of reduced gold nanoparticles on ceria nanocubes exposing the {100} surface plane, it is inferred that the gold nanoparticles on the ceria nanorod surface also have a low activity in such reactions. Although the finely dispersed Au clusters are thermally stable up to quite high temperature in line with earlier findings (Y. Guan and E. J. M. Hensen, Phys Chem Chem Phys 11:9578, 2009), the presence of gold nanoparticles results in their more facile agglomeration, especially in the presence of water (e.g., WGS conditions). For liquid phase alcohol oxidation, metallic gold nanoparticles are the active sites. In the absence of a base, the O-H bond cleavage appears to be rate limiting, while this shifts to C-H bond activation after addition of NaOH. In the latter case, the gold nanoparticles on the surface of ceria nanocubes are much more active than those on the surface of nanorod ceria.

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Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

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Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

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“…4,12 Interest is growing in the application of basic hydrotalcite (HT: Mg 6 Al 2 (OH) 16 The properties of hydrotalcites can be finetuned because of the possibility to act as cation-and anionexchangers of the Brucite layer and interlayer, respectively, their adjustable surface basicity and the ''memory effect'' of the layered structure. 17 In this communication, we report for the first time that the addition of transition metal cations to HTs provides excellent supports for AuNPs.…”

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“…[6][7][8][9][10][11] From the viewpoint of green chemistry, it is more desirable to develop bifunctional catalysts combining Au NP with a solid base support. 4,12 Interest is growing in the application of basic hydrotalcite (HT: Mg 6 Al 2 (OH) 16 of organic chemicals. It has been demonstrated that such Au/HT catalysts can be more active in the absence of base additives than other commonly used gold catalysts such as Au/TiO 2 , Au/CeO 2 and Au/Al 2 O 3 , suggesting synergy between AuNPs and basic sites of the HT.…”

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Aerobic oxidation of alcohols over hydrotalcite-supported gold nanoparticles: the promotional effect of transition metal cations

et al. 2011

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Chromium (III)-containing hydrotalcites show strong synergy with gold nanoparticles in achieving high activity in the aerobic oxidation of alcohols.Recently, considerable attention has been devoted to the application of supported gold nanoparticle (AuNP) catalysts in the selective aerobic oxidation of alcohols to replace toxic and stoichiometric metal oxide-based oxidation processes. 1The catalytic activity of supported AuNP catalysts depends not only on the size of the gold particles, but also on the nature of the gold-support interactions.1-7 A common feature of many AuNP catalysts employed for liquid-phase aerobic oxidation of alcohols is the need for bases such as NaOH and K 2 CO 3 to activate the reactant.6-11 From the viewpoint of green chemistry, it is more desirable to develop bifunctional catalysts combining Au NP with a solid base support. 4,12 Interest is growing in the application of basic hydrotalcite (HT: Mg 6 Al 2 (OH) 16 The properties of hydrotalcites can be finetuned because of the possibility to act as cation-and anionexchangers of the Brucite layer and interlayer, respectively, their adjustable surface basicity and the ''memory effect'' of the layered structure. 17 In this communication, we report for the first time that the addition of transition metal cations to HTs provides excellent supports for AuNPs. The resulting catalysts are very active for the aerobic oxidation of alcohols.The HT precursor (Mg 4 Al 2 (OH) 12 CO 3 ) was prepared by the homogeneous precipitation method using urea hydrolysis.

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Nanocatalysis in Water

Baig

Varma

2013

Metal‐Catalyzed Reactions in Water

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Basic metal carbonate supported gold nanoparticles: enhanced performance in aerobic alcohol oxidation

Cited by 53 publications

References 19 publications

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

Aerobic oxidation of alcohols over hydrotalcite-supported gold nanoparticles: the promotional effect of transition metal cations

Nanocatalysis in Water

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